JP2023502736A - Rotating Continuous Mulch for Improved Direct Air Capture of Carbon Dioxide (DAC+) - Google Patents

Abstract

A system and method for removing carbon dioxide from a carbon dioxide-containing gas mixture, the system comprising a group of carbon dioxide removal structures traveling along a closed curvilinear track. One location along the track is provided with a desorption or regeneration box through which each capture structure passes to be regenerated. Most of the CO2 removal structures are supplied with ambient air, or a mixture of ambient air and a small portion of the flue gas, and exhausted CO2 purified air. At least one such selected removal structure within each group is supplied with flue gas containing at least 4% by volume of CO2 at a position immediately prior to its entry into the capture structure. A method is provided for removing carbon dioxide from the atmosphere utilizing a system that operates similarly to the system described above. [Selection drawing] Fig. 1

Description

CAPTURE SYSTEM AND APPARATUS The present invention relates generally to systems and methods for removing greenhouse gases from the atmosphere, and more particularly to the initial capture of carbon dioxide from a gas stream comprising ambient air, followed by flue gas. A new and improved system and method for capturing carbon dioxide from at least one stream of containing gas. The present invention contemplates systems in which the sequence may include different sequences of carbon dioxide removal. The present invention further contemplates this second sequential step involving two or more streams of gas, including flue gas.

This invention is disclosed in U.S. Patent Application No. 13/098,370, filed April 29, 2011 (now U.S. Patent Application No. 8,500,855) and U.S. Patent Application No. 9,925,488. We provide an improvement to the system described. Systems and processes are presented that can be recognized as being able to be utilized for a wider range of uses than those disclosed in previous applications, particularly when further modified. The disclosure of this co-pending application, as modified by the new disclosure presented herein, is hereby incorporated by reference as if fully repeated.

At present, the focus is on achieving three conflicting energy goals: 1) Provide affordable energy for economic development. 2) Achieve energy security. 3) Avoid peculiar climate change caused by global warming. Here, avoiding the use of fossil fuels entirely for the remainder of this century is not feasible to ensure the energy needed for economic prosperity and to avoid energy shortages that could lead to conflict. Assume no.

There is little disagreement among respected scientists that increasing amounts of so-called greenhouse gases such as carbon dioxide (methane and water vapor are other major greenhouse gases) raise the average global temperature. .

It is also clear that the risks of climate change can only be eliminated by reducing the amount of carbon dioxide emitted by humans. It is also necessary to remove additional _CO2 from the atmosphere, known as direct air capture or direct air extraction (DAC). Through air extraction and the ability to reduce the amount of carbon dioxide in the atmosphere, emissions of other greenhouse gases such as methane (released into the atmosphere from both natural and human activities) that can cause climate change. can be compensated.

Especially in the last decade, among experts in the field, it has been suggested that the capture of carbon dioxide directly from the atmosphere, despite its low concentration, would at least slow the rise of so-called "greenhouse" gases in the atmosphere. It is becoming more common to think that it is economically feasible to It is now possible to efficiently extract _CO2 from the atmosphere under ambient conditions using suitably regenerable sorbent systems and moderately expensive but relatively low temperature stripping or regeneration processes, and such processes can be , can be extended and combined to remove _CO2 from flue gas mixtures mixed with bulk ambient air, and can remove _CO2 not _only from flue gas but also from the atmosphere. It is This allows net reduction of atmospheric CO ₂ at low cost and with high efficiency.

The present invention provides a DAC system and method for removing carbon dioxide from bulk carbon dioxide laden air with higher efficiency and lower capital costs ("CAPEX") and operating costs ("OPEX"). ”) at a lower overall cost, and provide further new and useful improvements.

SUMMARY OF THE INVENTION In accordance with the present invention, novel processes and systems are developed that utilize the assembly of multiple separate _CO2 capture structures. Each of the assemblies supports a substrate capture structure that may comprise a bed of substrate particles. The substrate capture structure reduces the rate of adsorption from ambient air or from any gas mixture being processed to remove _CO2 compared to the regeneration rate of the captured CO2 _- containing adsorbent. Combined with a single play box in ratio dependent ratios. In a preferred embodiment, the _CO2 trapping structure is supported on a substantially continuous closed loop track, preferably forming a closed curve, over which the _CO2 trapping structure is exposed to ambient air flow, or It is continuously moved longitudinally along the track while being exposed to a gas mixture containing most of the ambient air. Alternatively, the capture structure can be moved longitudinally back and forth along the open track.

At one location along the track longitudinal movement stops and one of the _CO2 capture structures is moved into a sealed box for processing, stripping the _CO2 from the adsorbent and regenerating the adsorbent. do. Once the sorbent is regenerated, the capture structure rotates around the track until the next _CO2 capture structure is positioned to enter the regeneration box, then all _CO2 capture structures are stopped from rotating. be. A refinement of the invention is to have at least one of the acquisition structures contain flue gas instead of ambient air, and preferably at least a majority of the other acquisition structures are supplied with ambient air. Most preferably, the last station before the regeneration box, i.e. the stage, is pure but pretreated flue gas or a mixture of flue gas and ambient air (referred to herein as carbonized flue gas). It is to receive a certain flue gas input.

The input flue gas velocity and concentration are independently controlled at the input, while the output is drawn by a fan which may use a separate manifold. Ideally, in some circumstances this could be a retrofit to a pure DAC unit. Additional _CO2 is added to preheat the adsorbent within the capture structure matrix prior to entering the regeneration box. Cooling of the capture structure substrate and adsorbent after desorption in the regeneration box remains unchanged, but the heat removed can be used differently since the array is already preheated before regeneration begins. Compared to separate DAC and carb units, this integrated approach has the following advantages:
1. Increase total _CO2 production per DAC plant by 30% to 50% (expected value), thereby reducing capital investment per metric ton.
2. Using a capital plant similar to the DAC reduces the capital cost of the flue gas capture component.
3. Less energy is used per metric ton of _CO2 produced. that is,
A. This is because the amine sites that bind _high concentrations of CO have a low heat of reaction (note that in this embodiment, not only adsorbents containing primary amines, but also other adsorbents, such as those containing secondary amines, or mixtures may be optimal).
B. This is because more _CO2 is produced for the same sensible heat.
C. This is because the heat from the flue is used to preheat the array.

There are three cases to consider.
1. A single case where the cogeneration unit is sized to supply the heat and power of the system installation.
2. Being connected to a larger cogeneration facility, the available heat and flue gas _CO2 is more than used for the DAC unit, resulting in excess electricity and heat being generated.
3. In the case of a negative carbon power plant that captures _CO2 from the power supply based on the need for removal of flue gas _CO2 and determines the size of the provided DAC (in this case, since the entire facility is negative carbon, The amount of flue gas _CO2 capture can be selected based on cost (eg, remove more _CO2 than the power plant emits).

It will be seen that the same design holds for the above three cases. The only change is the size of the combined heat and power plant. It is determined by the energy needs of the DAC in 1 above, by the energy needs of the particular application (compression, etc.) in 2 above, and by the size of the negative carbon power plant in 3 above.

It could also be argued that in a world trying to cut emissions, it would penalize net combustion installations by 10% of chimney emissions, giving a credit for the negative carbon produced. In this case, this embodiment can be a preferred embodiment both from the viewpoint of climate change and from the viewpoint of economy. In the process of this embodiment, pure flue gas is used at least at the last station of _CO2 capture just before regeneration.

Another preferred embodiment provides a feed comprising previously pretreated, ie partially entrapped, flue gas. For example, this flue gas has long been used in industries with large CO2 _- containing exhaust emissions from final or final capture structures, i.e. fuel-fired power plants, cement production plants, steel plants, etc. is the exhaust from a conventional _CO2 removal system of the type. Such flue gas pretreatment systems are useful for flue gas emissions from the combustion process of solids such as coal or liquids such as petroleum, which may contain particulate or non-particulate compounds that are toxic to the sorbent. This is especially important when dealing with

In such a system, a plant that produces steam for heating the regeneration chamber provides waste to be treated according to this improved invention. Such systems include, for example, a single plant whose primary purpose is to provide steam for regenerating the adsorbent. A second alternative is to use the plant primarily for heat transfer co-production with another product such as electric power plants, cement plants, steel mills, and oil refineries. A preferred example is a combined heat and power plant for the production of fuel from the _CO2 produced from the plant of the invention. A further preferred example is a cogeneration plant producing fuel from _CO2 intended for sale or use elsewhere.

If the adjacent plant is a power plant, the products of that power plant include co-heated or surplus steam and electricity, at least a portion of which provide the steam or electricity required to operate the DAC plant. include. The combustion waste, i.e. flue gas, from such power plants is at least partially cleaned and then the waste is fed to the final stage of _CO2 capture just before entering the regeneration chamber. Additionally, as described above, the partially _CO2 -depleted waste can be used immediately before the capture structure, ie, at the eighth position, either alone or mixed with ambient air. Of course, if there is a single regeneration chamber with ten capture structures, the regeneration chamber is the tenth stage and the capture structure stage just before the capture structure enters the regeneration chamber is the ninth stage. The stage, and the stage before it, will be understood to be the eighth stage. Examples of structures suitable for the system are shown in the drawings and legend below.

Another preferred embodiment provides a _{CO2 -} containing feed comprising flue gas that has been partially pretreated to capture CO2. For example, the flue gas may be the exhaust from a final or final capture structure, or conventional _CO2 removal systems traditionally used in industries with large amounts of CO2 _- containing exhaust (fuel-burning power plants, cement manufacturing plants, (e.g. steel plants). Systems with such waste pre-treatment may be used to control emissions from combustion processes of solids such as coal, or liquids such as petroleum, containing particulates, solid or liquid particles, gases toxic to adsorbents, etc. This is especially important when dealing with

A further preferred embodiment is the situation where the plant produces fuel intended for sale or use elsewhere from the _CO2 produced from the DAC+ plant of the present invention.

Each capture structure is formed from a porous substrate having carbon dioxide adsorption sites on its surface, preferably amine groups, and most preferably amine groups with a high proportion of primary amines. As the capture structures move along the track, each capture structure adsorbs _CO2 from the moving gas stream until it reaches a closed regeneration box. According to this refinement, flue gas instead of ambient air is passed through _{each CO2} capture structure while it travels in the loop a few minutes before reaching the regeneration box. This can further improve the process.

However, as explained above, the present process invention is a low temperature (preferably ambient to 100° C.), semi-continuous process with unidirectional mass transport during each phase of the process. A further novel aspect of this process is that the reaction that captures _CO2 from the gas mixture occurs on a renewable material (in one preferred embodiment on aminopolymers) and is based on renewable materials, such as aminopolymer adsorbents. It preferably occurs impregnated in the material.

The sorbent-bearing capture structure, in preferred embodiments, comprises a monolithic substrate supported in turn by:
1. A framework that supports the substrate along a closed loop or open line along which the substrate travels during the _CO2 capture process. In one preferred embodiment, the substrate comprises a porous monolith having an adsorbent impregnated within the pores of the monolith;
2. Substrates in one preferred embodiment of the present invention include, for example, cordierite, mullite, silica, alumina, titania, silica mesocellular foam (MCF), and mesoporous-γ-alumina, as well as MCF or other such materials ceramic materials from mesoporous-gamma-alumina, metal oxides (e.g. silica, alumina, titania, or porous oxides of other metals, single or mixed) coated throughout the pores of sufficient structural strength and thermal resistance to be able to maintain its monolithic shape under satisfactory conditions during the _CO2 capture step or during regeneration of the adsorbent as described below. have Porous fiberglass, rigid polymeric plastics, or other materials that can be formed into desired shapes by extrusion, corrugating, crimping, 3D printing, or molding, or other known or developed procedures, if thermal conditions are less severe. Other porous materials may be used, such as structurally strong porous materials such as
3. Impregnated Adsorbent a. The most commonly used adsorbents are aminopolymers.
i. Polyethylenimine (PEI) is the adsorbent of choice for most people working in the field for the following reasons.
1. High activity at low _CO2 concentration, high amine density, large scale commercial availability.
2. However, it is limited by known oxidative decomposition at high temperatures.
ii. Other amino polymers can be used as adsorbents with varying degrees of primary, secondary, and tertiary amines, and varying backbone chemistries, molecular weights, degrees of branching, and additives. Other known polyamines useful as _CO2 adsorbents are polypropyleneamine, polyglycolamine, polypropyleneamine (vinylamine), and poly(allylamine), and their derivatives.
iii. Non-amino polymeric adsorbents should be considered as useful adsorbents.
1. Metal-organic frameworks, covalent organic frameworks, POMs, and other such materials are useful.
2. Non-Polymerizable Amine Adsorbents (“Ph-XX-YY”), Oligomers.
3. Improvements to the system have been combined with adsorbents for high stability (scavenging agents), activity (copolymers), accessibility (PEG), and many others known in the art or to be developed in the future. This can be achieved through the use of non-adsorptive additives.

It is contemplated by the present invention that contactors constructed from active adsorbents (eg, 3D printed) may also be used.

Analysis In general, a DAC removal system (“system”) operates by feeding (preferably pre-treated) flue gas to the final stage of _CO2 capture before each substrate enters the regeneration chamber. , captures the excess component FGCO ₂ from the flue gas per DAC cycle. This captures additional CO ₂ (“FG CO ₂ ”). This improves efficiency in the final stages and increases the amount of _CO2 captured during each cycle of the system. First, the capital investment per metric ton is reduced by 1/(1+FGCO ₂ ) compared to a pure DAC (without added flue gas). This is due to the increased _CO2 concentration in the flue gas compared to ambient air. The effect of increased concentration varies with adsorbent type. Also, the cost of additional equipment is avoided when treating air containing a small fraction of the flue gas at each stage.

If a combined heat and power plant burns M*(MMbtu) amounts of natural gas per year, the amount of energy M produced for heat and electricity is given by M=COGENE*M* and exits the flue The primary energy content is MF = (1-COGENE) x M*, the energy of which does not include the reaction energy when _CO2 is captured and the energy of water when it is condensed, and COGENE is the combined heat transfer unit energy efficiency. The flue gas _CO2 emissions, FT _CO2 per year, is _FTCO2 = 0.056 M*metric tons/year.

If the _CO2 is captured from the flue gas at the capture ECF efficiency, the amount of _CO2 captured from the flue gas per year is:
_FGCO2 = ECF x _FTCO2
The ratio DACCO2 between _FCCO2 and total air _CO2 captured per _year is the same as the ratio per cycle. For a DAC unit, this means capturing ₂ metric tons of DACCO per year where:
_DACCO2 = (l/ _FGCO2 ) x ECF x _FTCO2
Total CO ₂ captured (TCCCO ₂ ) is determined from:
TCCO ₂ =(l/FGCO ₂ +−l)×ECF×FTCO _2.
The amount of CO ₂ emitted is (1-ECF)FTCO ₂ . The entire plant will have minus carbon by the amount of (1/FGCO ₂ +1)×(ECF−1)FTCO ₂ .

For an ECF=0.9 (for air mixed with a small percentage of flue gas (“carburetor”)), this is 1.7 FTCO ₂ (FGCO ₂ =.S) to −0.8 FTCO ₂ (FGCO ₂ =1). This means that less _FGCO2 entering the system means more negative carbon in the plant, whereas more negative carbon in the plant means less Capex reduction. This is expected to result in a smaller capital investment for a larger percentage of flue gas captured, but a smaller overall plant for larger negative carbon.

If the cogeneration unit is sized only to provide heat and electricity for the DAC unit, its _CO2 is exhausted through the _CO2 removal system, and the total energy (heat and electricity) is For example, at 6MMbtu per metric ton, the plant is (1-0.9 x 6 x 0.056) minus carbon or about 0.7. This clearly agrees well with the case where FGCO ₂ equals 1. However, in the pure DAC case, no extra power is generated. This results in higher CAPEX costs and higher energy consumption per metric ton. So, for example, less CAPEX, less energy used for capture, more negative carbon, etc., this integrated embodiment is preferred.

The next thing to evaluate is how much less energy you need and therefore how much extra power you can produce. If MDAC is the energy required per metric ton of DAC production and MFG is the energy required to capture 1 metric ton of flue gas (for MFG, the excess of flue gas constituents is Assuming that there is no significant sensible heat component and the heat of reaction to liberate _CO2 is reduced), the total energy required to capture _CO2 per metric ton is given by:
MT _CO2 = ((1/ _FGCO2 ) x MDAC + MFG)/((1/ _FGCO2 } + l} = (MDAC + _FGCO2 x MFG}/(l + _FGCO2 })
This already saves energy per metric ton compared to the DAC case.
MDAC−MTCO ₂ =(MDAC−J\;1FG}FGCO ₂ /(l+FGCO ₂ }=(SHA+ΔHR}×(FGCO ₂ /(l+FGCO ₂ }})
where SHA is the total sensible heat and ΔHR is the reduction in the heat of reaction of the flue gas components. Electricity usage per metric ton is also reduced.

Moreover, if the heat of the flue gas can be used to preheat the array to provide half the SHA, there is a further reduction of 0.5 SHA. Note that this heat is generated from the flue gas stream and is therefore not normally used, so it does not reduce the production of electricity and is completely waste heat.

If the SHA is recovered after regeneration, 3/4 of the sensible heat can be recovered by heat exchange, as is done in a system of two regeneration boxes, for example, as described in US Pat. No. 9,925,488. It is possible in principle. It is possible to do so directly with the heat of the flue gas, but increasing the temperature may reduce the excess _CO2 captured (again there is a trade-off between capacity and kinetics) . Depending on the application, there may be the use of low heat, including preheating of the water to the combined heat transfer unit, but in a highly preferred embodiment, preheating occurs in the final stages of adsorption, so the best result is faster regeneration. can be

In this respect it should be noted that there is another degree of freedom in the design of the flue gas stage. That is, the velocity and concentration of the flue gas stream are selected and kept constant to match the velocity of the flue gas _CO2 with which the products are discharged. In general, high concentrations and low speeds are desired because low speeds make the DAC monolith look like a higher CPSI. If the monolith has 100 CPSI and has a damping index of 0.7 at 5 rn/s, then at 1 m/s the damping index will be 3.5. Another more general feature of this embodiment is that although the capture efficiency from the flue gas stream can be moderated, the overall result is still negative carbon. Determining the optimum efficiency parameters for each system needs to be empirically determined from the velocities and concentrations of the flue gas components being treated.

The remaining question, therefore, is whether there is sufficient available heat in the flue gas stream passing through the contactor to provide the necessary heat to preheat the substrate prior to regeneration. be. The heat required to preheat the array is provided by the heat produced by the condensed water, the heat of reaction of _CO2 captured from the flue gas stream, and the sensible heat of the flue gas stream as follows: obtain.
a. THF = total heat in flue gas = SHF + heat of condensation of water vapor (HFCW) in flue gas stream + reaction of _CO2 (HFRC) per metric ton of _CO2 captured at last station before regeneration heat

To give a very rough estimate of whether there is enough heat, assuming SHA is 2MM BTU _per metric ton of _CO2 , the overall heat required is: Assume a 6MM BTU that is about 30% of the energy emitted at one time.
a. _CO2 capture is only up to _½ of the total CO2 recovered and will not add much due to the low heat of reaction.
b. SHF = sensible heat in flue gas per metric ton of _CO2 captured = (1-COGENE)M*. When in the 70% range of COGENE, 30% goes up the flue. Now assume that 1/4 of that heat is available (by cooling from 200°C to 50°C). This can be about 1/2 of what is needed.

However, the latent heat from available water vapor in the flue gas entering the last stage of the _CO2 capture stage will be sufficient to preheat the _CO2 capture unit before entering the regeneration box. Therefore, in another preferred embodiment, the hot flue gas is cooled by evaporating water so that the input flue gas stream has a delta T (e.g. 70°C) above the final temperature, e.g. 60°C. It is possible. However, the water vapor content of the flue gas was high, containing more than the amount of latent heat required to raise the substrate ("SA") temperature to 60°C. Note that in this case preheating is done in 90 seconds. Assuming a velocity of 1 m/s, the flue gas generally contains at least about 10% water, which corresponds to 30 seconds of pure steam input at 300 cm/s. This is clearly excessive. However, the excess water produced in this way would be a valuable by-product in places such as desert areas where water is expensive, for example in the southwestern United States or desert areas in Africa or Asia. If the SA enters the regeneration box at 60° C., it is possible to reduce the pressure to 0.2 bar without significantly cooling the regeneration box. In practice, lowering the pressure further may result in further cooling, but water vapor may be used to sweep away the trapped flue gas.

Once sealed in the regeneration box, the adsorbent is treated, for example by heating with steam, to remove the _CO2 from the adsorbent and regenerate the adsorbent. The extracted _CO2 is taken out of the box and captured. The capture structure with regenerated sorbent is then moved out of the sealed box and moved to another position to adsorb more _CO2 until the next capture structure moves into the regeneration box. capture structure along the track. In the strip/regenerate position, the capture structure can be moved into a box placed above or below the slope of the track, or the capture structure can be moved into the box at the same slope level as the track and the capture structure A box may be installed to form a seal with the body. Some of these alternatives are further defined below and illustrated in the accompanying drawings.

In instances where the regeneration box is below or above the gradient, the system must include a subsystem for raising or lowering the capture structure. A system where the recycle box is on the slope of the track requires a satisfactory sealing arrangement to provide seals along the sides and along the top and/or bottom.

_CO2 Adsorption and Removal Step The premise of this process is the adsorption of _CO2 from the atmosphere by passing air or a mixture of air and tail gas through an adsorbent bed, preferably at or near ambient temperature. Once the _CO2 is adsorbed on the adsorbent, the _CO2 needs to be captured and the adsorbent regenerated. The latter step can be performed by heating the adsorbent with steam in a sealed containment box to release the _CO2 and regenerate the adsorbent. _CO2 is recovered from the box and the adsorbent is then available to re-adsorb _CO2 from the atmosphere as it leaves the regeneration box.

It is well known that most commercially available adsorbents are readily decomposed and thus deactivated when exposed to air above a certain temperature. Therefore, in many cases the adsorbent on the substrate must be cooled before the capture structure leaves the regeneration box and is returned to the air stream.

In another preferred embodiment of the process of the present invention, the flue gas, preferably in purified form after removal of any particulate solid or liquid material, and any gaseous material toxic to the adsorbent, is treated with a capture structure is flowed through the capture structure just prior to entering the regeneration chamber. This flue gas treatment step is preferably carried out in a closed chamber. Thereby, the pretreated flue gas cannot escape into the environment prior to passing through the major surface of the porous substrate within the capture structure.

In general, the duration of _CO2 adsorption from ambient air is longer than the adsorption time from flue gas, and the concentration of _CO2 is much higher. In current production of sorbents, this difference requires roughly ten times the duration of adsorption when treating ambient air compared to the time required for CO ₂ release and sorbent regeneration. Therefore, based on the use of polyethyleneimine sorbents, systems with 10 trapping structures and a single regeneration unit are taken as the current basis for each rotating system. If the performance of the adsorbent improves over time, the ratio of adsorption to desorption time, and thus the number of capture structures required for the system, may decrease.

Especially when higher loading sorbent embodiments are used, 1 hour adsorption times are feasible, thus requiring 1 regeneration box to accommodate only 5 capture structures. . In addition, the relative treatment times vary with the concentration of _CO2 in the treated gas mixture, with higher _CO2 contents resulting in shorter adsorption times relative to regeneration times. For example, by mixing combustion waste (“flue gas”) with ambient air through a gas mixer, or “carburetor,” the mixture will have a significantly higher _CO2 concentration than air, but pure flue gas has a significantly lower concentration than

In order to more completely and reliably remove _CO2 from the flue gas, the waste from the ninth or final stage just before regeneration is returned into the second chamber. Preferably, the previous stage, ie the eighth stage of the adsorption cycle of the capture structure, is returned.

In all of the above embodiments, the process of the present invention remains a low temperature (ie, ambient temperature, below 100° C.) batch process, with unidirectional mass transport at each stage of the process.

The chemical and physical activity within the trapping structure and the mechanism of the trapping structure and regeneration chamber during at least the first seven stages of the adsorption cycle and the regeneration cycle within the sealed box are described in U.S. Pat. No. 10,413. , 866 and 10,512,880. The disclosures of these patents are hereby incorporated by reference as if fully repeated, as modified by the new disclosures presented herein. In the system according to the invention, each rotating system provides one sealed regeneration box for each group of rotating capture structures. The number of capture structures depends on the relative time to achieve desired adsorption and desired regeneration. Furthermore, in certain preferred embodiments, two of the rotating systems are spatially related in a suitable relationship and temporally coupled to allow interaction of the regeneration boxes for the two rotating capture structure systems. It has been found that by operating systematically, greater efficiency and lower costs are achieved. By offsetting the time each enters the regeneration box, regeneration in the first box results in the second being preheated with the residual heat of the first and entering its regeneration box. This also allows for efficient cooling of the regenerated capture structure before returning it to its adsorption cycle on the rotating track.

This interaction between the regeneration boxes is achieved according to the invention by reducing the pressure of the first box system, so that the steam and water remaining in the first box after the release of _CO2 evaporates. , the system cools to the saturation temperature of the vapor at its reduced partial pressure. Additionally, as described below, the heat released in this process is used to preheat the second sorbent capture structure, resulting in approximately 50% sensible heat recovery and energy and beneficially affect water use. This concept can be utilized even if oxygen-tolerant adsorbents are utilized. The use of less oxygen sensitive adsorbents at higher temperatures will result in improved performance over time. The high concentration of direct flue gas injection in at least the final stage immediately before the regeneration box, and possibly in one or more stages before it, leads to a high concentration of _CO2 adsorbed on the adsorbent and an exothermic heat of the adsorption reaction. It will be appreciated that the adsorbent and substrate will be hotter depending on the nature. This makes it possible to avoid the need to optionally reduce the pressure in the regeneration chamber to vacuum when dealing with ambient air only processing or mixing with a small percentage of flue gas. Become.

As discussed in previous patents, the adsorbent capture structure is preferably cooled prior to exposure to air to avoid deactivation by oxygen in the air. Utilizing adsorbents and their derivatives with greater resistance to thermal decomposition, such as poly(allylamine) and poly(vinylamine) among polyamines, as described in US patent application Ser. No. 14/063,850 can do. Cooling can be achieved, if desired, by lowering the system pressure in the regeneration box to lower the vapor saturation temperature. This has been shown to be effective in eliminating the adsorbent deactivation problem as it lowers the temperature of the system. As a result, a significant amount of energy is removed from the first capture structure that is cooled during the depressurization step. Each time the _CO2 -bearing substrate that has completed the _CO2 adsorption stage enters the _second regeneration box, it needs to be heated to release the CO2 and regenerate the adsorbent. This heat can be supplied solely by atmospheric pressure steam supplied to the regeneration box, but this is an extra operating cost. To minimize this operating cost, a two-bed design concept was developed. In this concept, the first regeneration box being cooled by lowering the system pressure (and thus the vapor saturation temperature) in the first regeneration box, as described in US Pat. No. 10,512,880. The heat removed from the box is used for at least partial preheating of the CO2 _- containing substrate to be regenerated in the second regeneration box. Thus, steam usage is reduced by using heat from cooling the first box to increase the temperature of the second box. The remaining heat load of the second box is accomplished by adding steam, preferably at atmospheric pressure. This process is repeated for other rotating capture structures entering and exiting the two regeneration boxes, greatly improving the thermal efficiency of the system.

Some acronyms above may be defined as follows.
FG- _CO2 = ratio of _CO2 to trapped air _CO2 capture per cycle which is flue gas DA. _CO2 = amount of air _CO2 captured per cycle FGCAPEX = pure carb run Flue gas operating costs in the form, i.e., if a mixture of ambient air and flue gas is supplied to each capture structure, M* = total natural gas burned in MMBTu M = available heat and Electricity generated COGENE = combined heat and power efficiency = M/M*
_FGCCO2 = flue gas _CO2 captured per year
DACCO2 = air _CO2 captured per _year
FTCO ₂ == total flue gas CO ₂ produced with J\11* natural gas burned
MTCO2 = total _CO2 captured per year = total _CO2 from flue gas and air captured per _year
ECF = efficiency of flue gas capture MDAC = energy per metric ton of trapped air _CO2 MFG = energy per metric ton of trapped flue gas _CO2 SHA = sensible heat of the monolith array delta HR = Difference in heat of reaction between DAC CO ₂ site and flue gas CO ₂ site THF = total heat source in flue gas steam - sensible heat + CO ₂ reaction heat + water condensation heat - (Natural gas heat value is not constant please note)

These and other features of the present invention are set forth in, or are apparent from, the following detailed description and accompanying drawings.

FIG. 2 is a schematic top view of a pair of rotating multi-capture structure systems interacting to remove carbon dioxide from the atmosphere, for each loop and each group of capture structures, according to an exemplary embodiment of the present invention; Gradient level regeneration chambers are shown with two capture structures immediately upstream of each of the regeneration chambers shown within sealed housings that supply cleaned flue gas to the capture structures. It has a sealed conduit for

FIG. 2 is a schematic illustration of a pair of regeneration chambers for removing carbon dioxide from the capture structure of FIG. 1, including several inlet and outlet conduits connected to one of the chambers and a sealing conduit connecting the two A connecting conduit is shown.

FIG. 4 is a schematic of the regeneration chamber and flue gas trapping structure on each of the adjacent loops showing each chamber and the piping system configuration between the chambers.

Figures 13A-13C are schematic elevational views respectively showing the fans relatively stationary and rotating with each capture structure;

5 is a schematic side view of the dual induction shaft fan and plenum design of FIG. 4; FIG.

1 is a schematic elevational view of one of the interacting pairs of a rotating multi-capture structure system with track-level regeneration chambers for removing carbon dioxide from the atmosphere and flue gas streams for _CO2 capture; FIG. Figure 2 shows two capture structure housings just before processing.

1 is a conceptual diagram showing the general operation of this system between the final adsorption stage and the _CO2 desorption regeneration step, showing a system in which all of the adsorption stages treat ambient air; FIG.

1 is a conceptual diagram showing the general operation between the final adsorption flue gas stage and the _CO2 desorption regeneration step of one of the inventively preferred embodiments of the system, which in this embodiment is referred to as "desorption The last adsorption stage immediately upstream of the unit, e.g. the 9th stage, receives flue gas pure or mixed with ambient air, the next preceding stage, e.g. exhaust, a mixture of that exhaust and ambient air, or ambient air only, depending on the composition of the ninth stage exhaust.

FIG. 2 is a conceptual diagram showing the general operation between the final adsorption mixed air flue gas stage and the _CO2 desorption and regeneration step of another preferred embodiment of the present invention of the system, in this embodiment: A final adsorption stage, for example the ninth stage, immediately upstream of the "desorption unit" receives flue gas mixed with ambient air.

within the desorption unit or out of the flue gas adsorption unit housing as each of the housings is at a graded level and each capture structure moves along the track and each capture structure enters each housing. FIG. 11 shows an example of a seal extending around all sides of each capture unit in one; FIG.

More Detailed Description of the Present Embodiment of the Invention A simplified depiction of the design of a system that performs these operations described above is shown in FIGS. 1-6. A detailed description of the maneuvers and ancillary equipment required are described below and are similar to those shown in common U.S. Pat. Nos. 10,413,866 and 10,512,880. .

In this embodiment, there are ten "capture structures". The capture structures are preferably, but not exclusively, placed in a decagonal configuration and placed on substantially circular or arcuate tracks. There are two substantially circular (or oval)/decagonal assemblies associated with each processing unit and they interact as shown. In this preferred embodiment, air is forced through the capture structure by an induced draft fan located inside the capture structure. At one location, the capture structures are located adjacent to a single sealed chamber box into which each capture structure is inserted as it moves along the track for processing. In a closed regeneration chamber box they are heated to a temperature below 130°C, more preferably below 120°C, optimally below 100°C, preferably with treated hot steam, releasing _CO2 from the adsorbent. Regenerate the adsorbent. Alternatively, the regeneration chamber can be above or below the gradient. In this embodiment, the _CO2 adsorption time by the capture structure is preferably ten times longer than the adsorbent regeneration time.

While it is preferred to use a porous monolithic substrate in the capture structure, it is possible to use porous particles, i.e. a stationary bed of particulate material, supported within a frame on the capture structure. Please understand. In either case, the porous substrate preferably supports an amine sorbent for _CO2 when the particle capture structure has the same pore volume as the monolithic capture structure for supporting the sorbent.

The schematic diagram illustrates the basic operating concept of the system according to the invention. There are ten "capturing structures" 21,22 each mounted in a decagonal assembly configuration and movably supported on circular tracks 31,33. There are two circular/decagonal assemblies, A and B, associated with each processing unit, which interact. Air or flue gas is forced through each of the capture structures 21, 22 by induced draft fans 23, 26 located radially inward of each of the decagon assemblies and out of the system from the inner perimeter of each capture structure. Inducing a flow of exhaust gas in the away direction. At one position along the tracks 31,33 the capture structures 21,22 are adjacent to the closed recycle boxes 25,27 and the capture structures 22,22 make one revolution about the track. After it is completed, it is inserted into it for playback processing.

Thus, as shown in Figures 1 and 2, the first capture structure 21 is rotated to a position within the regeneration box 25 for processing. It is for the regeneration box 25 on the gradient. When the capture structures are in position within the play box 25, movement along the track is stopped for all of the capture structures. Alternatively, continue by increasing the track diameter and trapping structure and by having a suitable sealing system on the regeneration box and optional flue gas adsorption housing (121, 221, 122, 222). movement becomes possible. When the capture structures 21, 22 are regenerated and all of the capture structures are displaced, the regenerated capture structures are displaced from the regeneration boxes 25, 27 as shown in FIG. After the structures 21, 22 have treated the flue gas, they can be moved. This process is repeated substantially continuously. In the preferred embodiment shown in the drawings, one or more of the capture structures on each track move from the flue gas adsorption housing (121, 221, 122, 222). The timing preferably coincides with the timing of flue gas desorption. Alternatively, movement of the capture structure may be stopped each time the capture structure enters the regeneration box and one or more flue gas adsorption housings (121, 221, 122, 222). Transfer is then resumed when desorption and flue gas adsorption are complete.

However, as explained above, the present process invention is a low temperature (preferably ambient to 100° C.), semi-continuous process with unidirectional mass transport during each phase of the process. In a further novel aspect of this process, the reaction that captures _CO2 from the gas mixture takes place on a renewable material (in one preferred embodiment on aminopolymers) and the renewable material, e.g. It preferably occurs impregnated within the base material.

In preferred embodiments, the sorbent-bearing capture structures comprise a monolithic substrate that is in turn supported by a framework to form each capture structure.

Although the two decagon ring assemblies are interoperable, the capture structures for each decagon ring are moved in and out of their desorption/regeneration boxes at slightly different times, as described below. This makes it possible, for example, to pass heat between the boxes 25 and 27 to preheat the other box, for example the regeneration box 27, when the regeneration in the box 25 is completed. This saves heat at the start of regeneration and reduces the cost of cooling the capture structure after regeneration.

Three locations are available for the regeneration boxes 25, 27: above or below the rotating capture structure, or at a slope level, which does not allow continuous movement. See U.S. Pat. Nos. 10,413,866 and 10,512,880.

Regeneration chambers 32l, 327 are mounted on the gradient of the rotating capture structure assembly. The box is similarly installed on a slope with adequate accessibility for maintenance and process piping. Suitable mutual sealing surfaces are placed on the box and on each capture structure such that when the capture structure is moved into position within the box, the movement is upward into the regeneration box on the rise. Or the boxes 322, 327 are sealed whether downward into the regeneration box below the grade or straight into the regeneration box on the grade. The same is true for embodiments in which the flue gas adsorption housing (121, 221, 122, 222) can be on-grade or below or above the slope. There is also an optional closed chamber for the immediately preceding position along the track to feed flue gas or partially cleaned flue gas into the capture structure.

In all cases, the ancillary equipment (pumps, control systems, etc.) is preferably installed on the slope inside or outside the circumference of the track supporting the rotating capture structure assembly 29 .

The regeneration box and housing may be installed at different levels in particular situations without departing from the concept or scope of the present invention.

An alternative design within the scope of the present invention provides a system in which a pair of regeneration boxes, chambers 25, can move along a track. This is optimal if the track design allows for reciprocating motion by the capture structure along a straight track so that the play boxes 25 are not widely separated. Compared to existing disclosed devices in the prior art, this is as follows.
Minimize structural steel.
Locate all major equipment at grade level, except for the regeneration box, which serves only as a containment vessel.
Ensure that if the box is at a different level than the track, it does not interfere with the air flow to the capture structure.
Rotate all of the capture structures to prevent movement of the larger multi-unit system moving them into the regeneration box.
It allows the two regeneration boxes to be adjacent with a minimal gap to allow for the desired heat exchange for increased efficiency.

Mechanical actions with the necessary machinery and power include:
Rotating the two sets of capture structure assemblies about substantially circular tracks on the support structure and precisely positioning the components to positions where the capture structures are stopped, the capture structures are placed in the regeneration box and Securely and freely moves in and out of any flue gas adsorption housing.
The capture structure or substrate alone is removed, the capture structure is inserted into the regeneration box, the capture structure is removed from the regeneration box, and the capture structure is reinserted in its position on the track assembly. All of these movements occur vertically or alternatively as part of a horizontal rotational movement on the track. The capture structure and regeneration box are designed such that for vertically movable capture structures there is a substantially airtight seal between the top or bottom of each of the capture structures and the support structure of the box. be done. Seals can be on the sides as well as on the top and bottom for slopes of such regeneration boxes or flue gas adsorption housings. Alternatively, there may be a sealed door that closes when the capture structure moves into the regeneration box or flue gas adsorption housing. Examples of several conceptual designs of such seals are shown in the previously issued US Eisenberger patent and FIG. 10 of this application.

In all cases of one preferred embodiment, referring to FIGS. 1-9, the capture structure 21-1 (Ring A) is rotated into position and then regenerated or detached for processing, box 25. is moved to The pressure in the desorption box 25 (which houses the capture structure 21-1, ring A) is reduced to below 0.2 bar, for example using a vacuum pump 230. Box 25 is heated with steam at atmospheric pressure via line 235 . CO ₂ is produced from capture structure 21-1 and is removed via outlet piping 237 from box 25 for CO ₂ and condensate separated on condenser 240 (Fig. SA). Capture structure 22-1 (Ring B) is then placed in Box 27 (Ring B) while Box 25 is being processed, as described above (FIG. 5B). The steam supply to box 25 is stopped and the _CO2 and condensate outlet lines are isolated. Boxes 25 and 27 are connected by opening valve 126 in connecting tubing 125 (Fig. SC).

The pressure within box 27 is reduced using vacuum pump 330 associated with box 27 . This reduces the system pressure in both boxes and draws the residual vapor and inert elements in box 25 through box 27 and then to the vacuum pump. This cools the box 25 (and therefore the trapping structure 21-1, ring A) to a lower temperature (i.e., the saturation temperature at the partial pressure of the vapor in the box) such that the trapping structure 21-1 Reduces the potential for oxygen deactivation of the adsorbent when placed back into the air stream. This process also preheats box 27 (and therefore capture structure 22-1, ring B) from ambient temperature to saturation temperature at the partial pressure of the vapor in box 250. FIG. Thus, energy is recovered and the amount of atmospheric pressure steam required to heat the second box 27 (capture structure 22-1 ring B) is reduced (Fig. SD). As the vacuum pump 330 reduces the pressure in boxes 25 and 27, the temperature of the first box 25 drops (from approximately 100°C to some intermediate temperature) and the temperature of the second box 27 drops (from the ambient temperature to the same intermediate temperature). CO ₂ and inert gases are removed from the system by vacuum pump 330 .

A valve between the first box 25 and the second box 27 is closed to isolate the boxes from each other. The capture structure 21-1 ring A is cooled to a temperature below that at which oxygen deactivation of the adsorbent is a concern when the capture structure is placed back into the air stream. Because the second box 27 and the capture structure 22-1, ring B are preheated, the amount of steam required to heat the box and capture structure is reduced (Fig. 5E). Capture structure 21-1 ring A is then moved into the capture structure assembly. The ring A capture structure assembly is rotated by one capture structure, then capture structure 21-2 ring A is inserted into box 25 ready for preheating. Box 27 is heated with atmospheric steam and the stripped _CO2 is recovered (Fig. 5F).

When the second box 27 (which houses the capture structure 22-1 ring B) is fully regenerated, the steam supply to box B is isolated and the _CO2 and condensate lines are connected using valves 241, 242. separated by The valve 126 between the first box 25 and the second box 27 is opened and the pressure in boxes 25,27 is reduced using the vacuum pump 230 system for box 25. The temperature of the second box 27 (and hence the trapping structure 22-1, ring B) is reduced (see 5 above). The temperature of the first box 25 (which houses the capture structure 21-2, ring A) is increased (see 5 above) (FIG. 5G). A vacuum pump 230 reduces the pressure in boxes 25,27. The temperature in box 25 drops (from approximately 100°C to some intermediate temperature). The temperature in box 27 rises (from ambient to the same intermediate temperature). CO ₂ and inert gases are removed from the system by vacuum pump 230 . Capture structure 22-1, ring B, is moved back into the ring assembly and the assembly rotates one bed. Capture structure 22 - 2 , ring B, is then inserted into box 27 . Box 25 (containing capture structure 21-2 ring A) is heated with atmospheric steam to release CO ₂ and regenerate the adsorbent (FIG. 5H). Preheating of box 27 then takes place as described above. This process is repeated for every bed as the decagon rotates many times.

When dealing with the preferred embodiment shown in Figure 8, in which both rings comprise a pair of flue gas adsorption housings just before entering the regeneration box, a supply of pretreated flue gas is preferably provided. For example, the ninth adsorption stage immediately prior to the regeneration box contains pretreated flue gas, or a mixture of pretreated flue gas and ambient air, typically having about 10-15% CO ₂ . either supplied. The exhaust from that stage can contain, for example, 2-8% CO ₂ . Preferably, when the upper range of _CO2 is vented, most preferably the exhaust gas is further adsorbed through the housing of the immediately preceding desorption stage to reduce the exhaust gas to a suitable level for venting to the atmosphere.

Preferred Design Parameters The current preferred basic principles for system design are as follows.
Weight of each captured structure to move:
1,500-10,000lbs. (including support structure)
Approximate bed size: Width: 5-6 meters Height: 9-10 meters Depth: 0.15-1 meter

It should be noted that the size of the capture structures may be adjusted depending on the specific conditions and desired or achievable processing parameters at each pair of geographic locations in the system.

For a system with 10 capture structures in each decagonal ring, the preferred outer system size of circular/decagonal structures is about 15-17 meters, preferably about 16.5 meters. The capture structure support structures may be driven individually along the track by, for example, electric motors and drive wheels. Alternatively, the support structure may be fixed to a single large motor that is used to drive specific locations along the track and all structures around the track and closed loop. In either case, the play box is placed in one location and all of the structures can stop their movement when one of the support structures is placed to be moved into the play box. . The economics of a single drive motor or engine, or multiple drive motors or engines, depends on many factors such as location and whether the drive is accomplished by an electric motor or by several fuel-driven engines. Dependent. The nature of the drive unit per se is not a primary feature of the invention and many are well known to those skilled in the art. Examples of suitable engines include, for example, internal or external combustion or gas pressure driven engines, process steam engines, or hydraulic or pneumatic engines operating using the Stirling engine cycle.

If the regeneration box is installed above track level, the top is approximately 20 meters above track level. If the regeneration box is installed below the slope of the track, the top of the box is just below the slope of the track. The box on the gradient is placed at a minimum height above the top of the trapping structure in order to completely contain the trapping structure within the box during regeneration.

If the regeneration box is not on an incline, the lift system for moving the capture structure into and out of the regeneration box will move in and out of the box during a period within the range of 30 seconds to i20 seconds, preferably 30 seconds to 45 seconds. should be able to achieve a transfer of Shorter periods allow greater flexibility in processing parameters. It is recognized that moving large capture structures has certain inherent mechanical limitations. One advantage of having the play box on a gradient is that no vertical movement is required. The capture structure simply rotates and seals into the box as part of the rotational movement, thus avoiding the vertical movement, lost time, and additional capital cost of the elevator. In either case, the two edges of the capture structure are solid and form a seal with the edge of the regeneration box.

U.S. Patent Application No. 13/098,370 (now U.S. Patent Application No. 8,500,855) U.S. Patent Application No. 9,925,488

CAPTURE SYSTEM AND APPARATUS The present invention relates generally to systems and methods for removing greenhouse gases from the atmosphere, and more particularly to the initial capture of carbon dioxide from a gas stream comprising ambient air, followed by flue gas. A new and improved system and method for capturing carbon dioxide from at least one stream of containing gas. The present invention contemplates systems in which the sequence may include different sequences of carbon dioxide removal. The present invention further contemplates this second sequential step involving two or more streams of gas, including flue gas.

This invention is disclosed in U.S. Patent Application No. 13/098,370, filed April 29, 2011 (now U.S. Patent Application No. 8,500,855) and U.S. Patent Application No. 9,925,488. We provide an improvement to the system described. Systems and processes are presented that can be recognized as being able to be utilized for a wider range of uses than those disclosed in previous applications, particularly when further modified. The disclosure of this co-pending application, as modified by the new disclosure presented herein, is hereby incorporated by reference as if fully repeated.

At present, the focus is on achieving three conflicting energy goals: 1) Provide affordable energy for economic development. 2) Achieve energy security. 3) Avoid peculiar climate change caused by global warming. Here, avoiding the use of fossil fuels entirely for the remainder of this century is not feasible to ensure the energy needed for economic prosperity and to avoid energy shortages that could lead to conflict. Assume no.

There is little disagreement among respected scientists that increasing amounts of so-called greenhouse gases such as carbon dioxide (methane and water vapor are other major greenhouse gases) raise the average global temperature. .

It is also clear that the risks of climate change can only be eliminated by reducing the amount of carbon dioxide emitted by humans. It is also necessary to remove additional _CO2 from the atmosphere, known as direct air capture or direct air extraction (DAC). Through air extraction and the ability to reduce the amount of carbon dioxide in the atmosphere, emissions of other greenhouse gases such as methane (released into the atmosphere from both natural and human activities) that can cause climate change. can be compensated.

Especially in the last decade, among experts in the field, it has been suggested that the capture of carbon dioxide directly from the atmosphere, despite its low concentration, would at least slow the rise of so-called "greenhouse" gases in the atmosphere. It is becoming more common to think that it is economically feasible to It is now possible to efficiently extract _CO2 from the atmosphere under ambient conditions using suitably regenerable sorbent systems and moderately expensive but relatively low temperature stripping or regeneration processes, and such processes can be , can be extended and combined to remove _CO2 from flue gas mixtures mixed with bulk ambient air, and can remove _CO2 not _only from flue gas but also from the atmosphere. It is This allows net reduction of atmospheric CO ₂ at low cost and with high efficiency.

The present invention provides a DAC system and method for removing carbon dioxide from bulk carbon dioxide laden air with higher efficiency and lower capital costs ("CAPEX") and operating costs ("OPEX"). ”) at a lower overall cost, and provide further new and useful improvements.

SUMMARY OF THE INVENTION In accordance with the present invention, novel processes and systems are developed that utilize the assembly of multiple separate _CO2 capture structures. Each of the assemblies supports a substrate capture structure that may comprise a bed of substrate particles. The substrate capture structure reduces the rate of adsorption from ambient air or from any gas mixture being processed to remove _CO2 compared to the regeneration rate of the captured CO2 _- containing adsorbent. Combined with a single play box in ratio dependent ratios. In a preferred embodiment, the _CO2 trapping structure is supported on a substantially continuous closed loop track, preferably forming a closed curve, over which the _CO2 trapping structure is exposed to ambient air flow, or It is continuously moved longitudinally along the track while being exposed to a gas mixture containing most of the ambient air. Alternatively, the capture structure can be moved longitudinally back and forth along the open track.

At one location along the track longitudinal movement stops and one of the _CO2 capture structures is moved into a sealed box for processing, stripping the _CO2 from the adsorbent and regenerating the adsorbent. do. Once the sorbent is regenerated, the capture structure rotates around the track until the next _CO2 capture structure is positioned to enter the regeneration box, then all _CO2 capture structures are stopped from rotating. be. A refinement of the invention is to have at least one of the acquisition structures contain flue gas instead of ambient air, and preferably at least a majority of the other acquisition structures are supplied with ambient air. Most preferably, the last station before the regeneration box, i.e. the stage, is pure but pretreated flue gas or a mixture of flue gas and ambient air (referred to herein as carbonized flue gas). It is to receive a certain flue gas input.

The input flue gas velocity and concentration are independently controlled at the input, while the output is drawn by a fan which may use a separate manifold. Ideally, in some circumstances this could be a retrofit to a pure DAC unit. Additional _CO2 is added to preheat the adsorbent within the capture structure matrix prior to entering the regeneration box. Cooling of the capture structure substrate and adsorbent after desorption in the regeneration box remains unchanged, but the heat removed can be used differently since the array is already preheated before regeneration begins. Compared to separate DAC and carb units, this integrated approach has the following advantages:
1. Increase total _CO2 production per DAC plant by 30% to 50% (expected value), thereby reducing capital investment per metric ton.
2. Using a capital plant similar to the DAC reduces the capital cost of the flue gas capture component.
3. Less energy is used per metric ton of _CO2 produced. that is,
A. This is because the amine sites that bind _high concentrations of CO have a low heat of reaction (note that in this embodiment, not only adsorbents containing primary amines, but also other adsorbents, such as those containing secondary amines, or mixtures may be optimal).
B. This is because more _CO2 is produced for the same sensible heat.
C. This is because the heat from the flue is used to preheat the array.

There are three cases to consider.
1. A single case where the cogeneration unit is sized to supply the heat and power of the system installation.
2. Being connected to a larger cogeneration facility, the available heat and flue gas _CO2 is more than used for the DAC unit, resulting in excess electricity and heat being generated.
3. In the case of a negative carbon power plant that captures _CO2 from the power supply based on the need for removal of flue gas _CO2 and determines the size of the provided DAC (in this case, since the entire facility is negative carbon, The amount of flue gas _CO2 capture can be selected based on cost (eg, remove more _CO2 than the power plant emits).

It will be seen that the same design holds for the above three cases. The only change is the size of the combined heat and power plant. It is determined by the energy needs of the DAC in 1 above, by the energy needs of the particular application (compression, etc.) in 2 above, and by the size of the negative carbon power plant in 3 above.

It could also be argued that in a world trying to cut emissions, it would penalize net-combustion installations by 10% of chimney emissions, giving credit for the negative carbon produced. In this case, this embodiment can be a preferred embodiment both from the viewpoint of climate change and from the viewpoint of economy. In the process of this embodiment, pure flue gas is used at least at the last station of _CO2 capture just before regeneration.

Another preferred embodiment provides a feed comprising previously pretreated, ie partially entrapped, flue gas. For example, this flue gas has long been used in industries with large CO2 _- containing exhaust emissions from final or final capture structures, i.e. fuel-fired power plants, cement production plants, steel plants, etc. is the exhaust from a conventional _CO2 removal system of the type. Such flue gas pretreatment systems are useful for flue gas emissions from the combustion process of solids such as coal or liquids such as petroleum, which may contain particulate or non-particulate compounds that are toxic to the sorbent. This is especially important when dealing with

In such a system, a plant that produces steam for heating the regeneration chamber provides waste to be treated according to this improved invention. Such systems include, for example, a single plant whose primary purpose is to provide steam for regenerating the adsorbent. A second alternative is to use the plant primarily for heat transfer co-production with another product such as electrical power plants, cement plants, steel mills, and oil refineries. A preferred example is a combined heat and power plant for the production of fuel from the _CO2 produced from the plant of the invention. A further preferred example is a cogeneration plant producing fuel from _CO2 intended for sale or use elsewhere.

If the adjacent plant is a power plant, the products of that power plant include co-heated or surplus steam and electricity, at least a portion of which provide the steam or electricity required to operate the DAC plant. include. The combustion waste, i.e. flue gas, from such power plants is at least partially cleaned and then the waste is fed to the final stage of _CO2 capture just before entering the regeneration chamber. Additionally, as described above, the partially _CO2 -depleted waste can be used immediately before the capture structure, ie, at the eighth position, either alone or mixed with ambient air. Of course, if there is a single regeneration chamber with ten capture structures, the regeneration chamber is the tenth stage and the capture structure stage just before the capture structure enters the regeneration chamber is the ninth stage. The stage, and the stage before it, will be understood to be the eighth stage. Examples of structures suitable for the system are shown in the drawings and legend below.

Another preferred embodiment provides a _{CO2 -} containing feed comprising flue gas that has been partially pretreated to capture CO2. For example, the flue gas may be the exhaust from a final or final capture structure, or conventional _CO2 removal systems traditionally used in industries with large amounts of CO2 _- containing exhaust (fuel-burning power plants, cement manufacturing plants, (e.g. steel plants). Systems with such waste pretreatment include exhaust gases, such as particulates, solid or liquid particles, gases toxic to adsorbents, etc., emitted from combustion processes of solids such as coal or liquids such as petroleum. This is especially important when dealing with

A further preferred embodiment is the situation where the plant produces fuel intended for sale or use elsewhere from the _CO2 produced from the DAC+ plant of the present invention.

Each capture structure is formed from a porous substrate having carbon dioxide adsorption sites on its surface, preferably amine groups, and most preferably amine groups with a high proportion of primary amines. As the capture structures move along the track, each capture structure adsorbs _CO2 from the moving gas stream until it reaches a closed regeneration box. According to this refinement, flue gas instead of ambient air is passed through _{each CO2} capture structure while it travels in the loop a few minutes before reaching the regeneration box. This can further improve the process.

However, as explained above, the present process invention is a low temperature (preferably ambient to 100° C.), semi-continuous process with unidirectional mass transport during each phase of the process. A further novel aspect of this process is that the reaction that captures _CO2 from the gas mixture occurs on a renewable material (in one preferred embodiment on aminopolymers) and is based on renewable materials, such as aminopolymer adsorbents. It preferably occurs impregnated in the material.

The sorbent-bearing capture structure, in preferred embodiments, comprises a monolithic substrate supported in turn by:
1. A framework that supports the substrate along a closed loop or open line along which the substrate travels during the _CO2 capture process. In one preferred embodiment, the substrate comprises a porous monolith having an adsorbent impregnated within the pores of the monolith;
2. Substrates in one preferred embodiment of the present invention include, for example, cordierite, mullite, silica, alumina, titania, silica mesocellular foam (MCF), and mesoporous-γ-alumina, as well as MCF or other such materials ceramic materials from mesoporous-gamma-alumina, metal oxides (e.g. silica, alumina, titania, or porous oxides of other metals, single or mixed) coated throughout the pores of sufficient structural strength and thermal resistance to be able to maintain its monolithic shape under satisfactory conditions during the _CO2 capture step or during regeneration of the adsorbent as described below. have Porous fiberglass, rigid polymeric plastics, or other materials that can be formed into desired shapes by extrusion, corrugating, crimping, 3D printing, or molding, or other known or developed procedures, if thermal conditions are less severe. Other porous materials may be used, such as structurally strong porous materials such as
3. Impregnated Adsorbent a. The most commonly used adsorbents are aminopolymers.
i. Polyethylenimine (PEI) is the adsorbent of choice for most people working in the field for the following reasons.
1. High activity at low _CO2 concentration, high amine density, large scale commercial availability.
2. However, it is limited by known oxidative decomposition at high temperatures.
ii. Other amino polymers can be used as adsorbents with varying degrees of primary, secondary, and tertiary amines, and varying backbone chemistries, molecular weights, degrees of branching, and additives. Other known polyamines useful as _CO2 adsorbents are polypropyleneamine, polyglycolamine, polypropyleneamine (vinylamine), and poly(allylamine), and their derivatives.
iii. Non-amino polymeric adsorbents should be considered as useful adsorbents.
1. Metal-organic frameworks, covalent organic frameworks, POMs, and other such materials are useful.
2. Non-Polymerizable Amine Adsorbents (“Ph-XX-YY”), Oligomers.
3. Improvements to the system have been combined with adsorbents for high stability (scavenging agents), activity (copolymers), accessibility (PEG), and many others known in the art or to be developed in the future. This can be achieved through the use of non-adsorptive additives.

It is contemplated by the present invention that contactors constructed from active adsorbents (eg, 3D printed) may also be used.

Analysis In general, a DAC removal system (“system”) operates by feeding (preferably pre-treated) flue gas to the final stage of _CO2 capture before each substrate enters the regeneration chamber. , captures the excess component FGCO ₂ from the flue gas per DAC cycle. This captures additional CO ₂ (“FG CO ₂ ”). This improves efficiency in the final stages and increases the amount of _CO2 captured during each cycle of the system. First, the capital investment per metric ton is reduced by 1/(1+FGCO ₂ ) compared to a pure DAC (without added flue gas). This is due to the increased _CO2 concentration in the flue gas compared to ambient air. The effect of increased concentration varies with adsorbent type. Also, the cost of additional equipment is avoided when treating air containing a small fraction of the flue gas at each stage.

If a combined heat and power plant burns M*(MMbtu) amounts of natural gas per year, the amount of energy M produced for heat and electricity is given by M=COGENE*M* and exits the flue The primary energy content is MF = (1-COGENE) x M*, the energy of which does not include the reaction energy when _CO2 is captured and the energy of water when it is condensed, and COGENE is the combined heat transfer unit energy efficiency. The flue gas _CO2 emissions, FT _CO2 per year, is _FTCO2 = 0.056 M*metric tons/year.

If the _CO2 is captured from the flue gas at the capture ECF efficiency, the amount of _CO2 captured from the flue gas per year is:
_FGCO2 = ECF x _FTCO2
The ratio DACCO2 between _FCCO2 and total air _CO2 captured per _year is the same as the ratio per cycle. For a DAC unit this means capturing ₂ metric tons of DACCO per year where:
_DACCO2 = (l/ _FGCO2 ) x ECF x _FTCO2
Total CO ₂ captured (TCCCO ₂ ) is determined from:
TCCO ₂ =(l/FGCO ₂ +−l)×ECF×FTCO _2.
The amount of CO ₂ emitted is (1-ECF)FTCO ₂ . The entire plant will have minus carbon by the amount of (1/FGCO ₂ +1)×(ECF−1)FTCO ₂ .

For an ECF=0.9 (for air mixed with a small percentage of flue gas (“carburetor”)), this is 1.7 FTCO ₂ (FGCO ₂ =.S) to −0.8 FTCO ₂ (FGCO ₂ =1). This means that less _FGCO2 entering the system means more negative carbon in the plant, whereas more negative carbon in the plant means less Capex reduction. This is expected to result in a smaller capital investment for a larger percentage of flue gas captured, but a smaller overall plant for larger negative carbon.

If the cogeneration unit is sized only to provide heat and electricity for the DAC unit, its _CO2 is exhausted through the _CO2 removal system, and the total energy (heat and electricity) is For example, at 6MMbtu per metric ton, the plant is (1-0.9 x 6 x 0.056) minus carbon or about 0.7. This clearly agrees well with the case where FGCO ₂ equals 1. However, in the pure DAC case, no extra power is generated. This results in higher CAPEX costs and higher energy consumption per metric ton. So, for example, less CAPEX, less energy used for capture, more negative carbon, etc., this integrated embodiment is preferred.

The next thing to evaluate is how much less energy you need and therefore how much extra power you can produce. If MDAC is the energy required per metric ton of DAC production and MFG is the energy required to capture 1 metric ton of flue gas (for MFG, the excess of flue gas constituents is Assuming that there is no significant sensible heat component and the heat of reaction to liberate _CO2 is reduced), the total energy required to capture _CO2 per metric ton is given by:
MT _CO2 = ((1/ _FGCO2 ) x MDAC + MFG)/((1/ _FGCO2 } + l} = (MDAC + _FGCO2 x MFG}/(l + _FGCO2 })
This already saves energy per metric ton compared to the DAC case.
MDAC−MTCO ₂ =(MDAC−J\;1FG}FGCO ₂ /(l+FGCO ₂ }=(SHA+ΔHR}×(FGCO ₂ /(l+FGCO ₂ }})
where SHA is the total sensible heat and ΔHR is the reduction in the heat of reaction of the flue gas components. Electricity usage per metric ton is also reduced.

Moreover, if the heat of the flue gas can be used to preheat the array to provide half the SHA, there is a further reduction of 0.5 SHA. Note that this heat is generated from the flue gas stream and is therefore not normally used, so it does not reduce the production of electricity and is completely waste heat.

If the SHA is recovered after regeneration, 3/4 of the sensible heat can be recovered by heat exchange, as is done in a system of two regeneration boxes, for example, as described in US Pat. No. 9,925,488. It is possible in principle. It is possible to do so directly with the heat of the flue gas, but increasing the temperature may reduce the excess _CO2 captured (again there is a trade-off between capacity and kinetics) . Depending on the application, there may be the use of lower heat, including preheating of the water to the heat transfer co-generation unit, but in a highly preferred embodiment preheating occurs at the end of the adsorption, so the best result is faster regeneration. can be

In this respect it should be noted that there is another degree of freedom in the design of the flue gas stage. That is, the velocity and concentration of the flue gas stream are selected and kept constant to match the velocity of the flue gas _CO2 from which the products are discharged. In general, high concentrations and low speeds are desired because low speeds make the DAC monolith look like a higher CPSI. If the monolith has 100 CPSI and has a damping index of 0.7 at 5 rn/s, then at 1 m/s the damping index will be 3.5. Another more general feature of this embodiment is that although the capture efficiency from the flue gas stream can be moderated, the overall result is still negative carbon. Determining the optimum efficiency parameters for each system needs to be empirically determined from the velocities and concentrations of the flue gas components being treated.

The remaining question, therefore, is whether there is sufficient available heat in the flue gas stream passing through the contactor to provide the necessary heat to preheat the substrate prior to regeneration. be. The heat required to preheat the array is provided by the heat produced by the condensed water, the heat of reaction of _CO2 captured from the flue gas stream, and the sensible heat of the flue gas stream as follows: obtain.
a. THF = total heat in flue gas = SHF + heat of condensation of water vapor (HFCW) in flue gas stream + reaction of _CO2 (HFRC) per metric ton of _CO2 captured at last station before regeneration heat

To give a very rough estimate of whether there is enough heat, assuming SHA is 2MM BTU _per metric ton of _CO2 , the overall heat required is: Assume a 6MM BTU that is about 30% of the energy emitted at one time.
a. _CO2 capture is only up to _½ of the total CO2 recovered and will not add much due to the low heat of reaction.
b. SHF = sensible heat in flue gas per metric ton of _CO2 captured = (1-COGENE)M*. When in the 70% range of COGENE, 30% goes up the flue. Now assume that 1/4 of that heat is available (by cooling from 200°C to 50°C). This can be about 1/2 of what is needed.

However, the latent heat from available water vapor in the flue gas entering the last stage of the _CO2 capture stage will be sufficient to preheat the _CO2 capture unit before entering the regeneration box. Therefore, in another preferred embodiment, the hot flue gas is cooled by evaporating water so that the input flue gas stream has a delta T (eg 70°C) above the final temperature, eg 60°C. It is possible. However, the water vapor content of the flue gas was high, containing more than the amount of latent heat required to raise the substrate ("SA") temperature to 60°C. Note that in this case preheating is done in 90 seconds. Assuming a velocity of 1 m/s, the flue gas generally contains at least about 10% water, which corresponds to 30 seconds of pure steam input at 300 cm/s. This is clearly excessive. However, the excess water produced in this way would be a valuable by-product in places such as desert regions where water is expensive, for example in the southwestern United States or desert regions in Africa or Asia. If the SA enters the regeneration box at 60° C., it is possible to reduce the pressure to 0.2 bar without significantly cooling the regeneration box. In practice, lowering the pressure further may result in further cooling, but water vapor may be used to sweep away the trapped flue gas.

Once sealed in the regeneration box, the adsorbent is treated, for example by heating with steam, to remove the _CO2 from the adsorbent and regenerate the adsorbent. The extracted _CO2 is taken out of the box and captured. The capture structure with regenerated sorbent is then moved out of the sealed box and moved to another position to adsorb more _CO2 until the next capture structure moves into the regeneration box. capture structure along the track. In the strip/regenerate position, the capture structure can be moved into a box placed above or below the slope of the track, or the capture structure can be moved into the box at the same slope level as the track and the capture structure A box may be installed to form a seal with the body. Some of these alternatives are further defined below and illustrated in the accompanying drawings.

In instances where the regeneration box is below or above the gradient, the system must include a subsystem for raising or lowering the capture structure. A system where the recycle box is on the slope of the track requires a satisfactory sealing arrangement to provide seals along the sides and along the top and/or bottom.

_CO2 Adsorption and Removal Step The premise of this process is the adsorption of _CO2 from the atmosphere by passing air or a mixture of air and tail gas through an adsorbent bed, preferably at or near ambient temperature. Once the _CO2 is adsorbed on the adsorbent, the _CO2 needs to be captured and the adsorbent regenerated. The latter step can be performed by heating the adsorbent with steam in a sealed containment box to release the _CO2 and regenerate the adsorbent. _CO2 is recovered from the box and the adsorbent is then available to re-adsorb _CO2 from the atmosphere as it leaves the regeneration box.

It is well known that most commercially available adsorbents are readily decomposed and thus deactivated when exposed to air above a certain temperature. Therefore, in many cases the adsorbent on the substrate must be cooled before the capture structure leaves the regeneration box and is returned to the air stream.

In another preferred embodiment of the process of the present invention, the flue gas, preferably in purified form after removal of any particulate solid or liquid material, and any gaseous material toxic to the adsorbent, is treated with a capture structure is flowed through the capture structure just prior to entering the regeneration chamber. This flue gas treatment step is preferably carried out in a closed chamber. Thereby, the pretreated flue gas cannot escape into the environment prior to passing through the major surface of the porous substrate within the capture structure.

In general, the duration of _CO2 adsorption from ambient air is longer than the adsorption time from flue gas, and the concentration of _CO2 is much higher. In current production of sorbents, this difference requires roughly ten times the duration of adsorption when treating ambient air compared to the time required for CO ₂ release and sorbent regeneration. Therefore, based on the use of polyethyleneimine sorbents, systems with 10 trapping structures and a single regeneration unit are taken as the current basis for each rotating system. If the performance of the adsorbent improves over time, the ratio of adsorption to desorption time, and thus the number of capture structures required for the system, may decrease.

Especially when higher loading adsorbent embodiments are used, one hour adsorption times are feasible, thus requiring one regeneration box to accommodate only five capture structures. . In addition, the relative treatment times vary with the concentration of _CO2 in the treated gas mixture, with higher _CO2 contents resulting in shorter adsorption times relative to regeneration times. For example, by mixing combustion waste (“flue gas”) with ambient air through a gas mixer, or “carburetor,” the mixture will have a significantly higher _CO2 concentration than air, but pure flue gas has a significantly lower concentration than

In order to more completely and reliably remove _CO2 from the flue gas, the waste from the ninth or final stage just before regeneration is returned into the second chamber. Preferably, the previous stage, ie the eighth stage of the adsorption cycle of the capture structure, is returned.

In all of the above embodiments, the process of the present invention remains a low temperature (ie, ambient temperature, below 100° C.) batch process, with unidirectional mass transport at each stage of the process.

The chemical and physical activity within the trapping structure and the mechanism of the trapping structure and regeneration chamber during at least the first seven stages of the adsorption cycle and the regeneration cycle within the sealed box are described in U.S. Pat. No. 10,413. , 866 and 10,512,880. The disclosures of these patents are hereby incorporated by reference as if fully repeated, as modified by the new disclosures presented herein. In the system according to the invention, each rotating system provides one sealed regeneration box for each group of rotating capture structures. The number of capture structures depends on the relative time to achieve desired adsorption and desired regeneration. Furthermore, in certain preferred embodiments, two of the rotating systems are spatially related in a suitable relationship and temporally coupled to allow interaction of the regeneration boxes for the two rotating capture structure systems. It has been found that by operating systematically, greater efficiency and lower costs are achieved. By offsetting the time each enters the regeneration box, regeneration in the first box results in the second being preheated with the residual heat of the first and entering its regeneration box. This also allows for efficient cooling of the regenerated capture structure before returning it to its adsorption cycle on the rotating track.

This interaction between the regeneration boxes is achieved according to the invention by reducing the pressure of the first box system, so that the steam and water remaining in the first box after the release of _CO2 evaporates. , the system cools to the saturation temperature of the vapor at its reduced partial pressure. Additionally, as described below, the heat released in this process is used to preheat the second sorbent capture structure, resulting in approximately 50% sensible heat recovery and energy and beneficially affect water use. This concept can be utilized even if oxygen-tolerant adsorbents are utilized. The use of less oxygen sensitive adsorbents at higher temperatures will result in improved performance over time. The high concentration of direct flue gas injection in at least the final stage immediately before the regeneration box, and possibly in one or more stages before it, leads to a high concentration of _CO2 adsorbed on the adsorbent and an exothermic heat of the adsorption reaction. It will be appreciated that the adsorbent and substrate will be hotter depending on the nature. This makes it possible to avoid the need to optionally reduce the pressure in the regeneration chamber to vacuum when dealing with ambient air only processing or mixing with a small percentage of flue gas. Become.

As discussed in previous patents, the adsorbent capture structure is preferably cooled prior to exposure to air to avoid deactivation by oxygen in the air. Utilizing adsorbents and their derivatives with greater resistance to thermal decomposition, such as poly(allylamine) and poly(vinylamine) among polyamines, as described in US patent application Ser. No. 14/063,850 can do. Cooling can be achieved, if desired, by lowering the system pressure in the regeneration box to lower the vapor saturation temperature. This has been shown to be effective in eliminating the adsorbent deactivation problem as it lowers the temperature of the system. As a result, a significant amount of energy is removed from the first capture structure that is cooled during the depressurization step. Each time the _CO2 -bearing substrate that has completed the _CO2 adsorption stage enters the _second regeneration box, it needs to be heated to release the CO2 and regenerate the adsorbent. This heat can be supplied solely by atmospheric pressure steam supplied to the regeneration box, but this is an extra operating cost. To minimize this operating cost, a two-bed design concept was developed. In this concept, the first regeneration box being cooled by lowering the system pressure (and thus the vapor saturation temperature) in the first regeneration box, as described in US Pat. No. 10,512,880. The heat removed from the box is used for at least partial preheating of the CO2 _- containing substrate to be regenerated in the second regeneration box. Thus, steam usage is reduced by using heat from cooling the first box to increase the temperature of the second box. The remaining heat load of the second box is accomplished by adding steam, preferably at atmospheric pressure. This process is repeated for other rotating capture structures entering and exiting the two regeneration boxes, greatly improving the thermal efficiency of the system.

Some acronyms above may be defined as follows.
FG- _CO2 = ratio of _CO2 to trapped air _CO2 capture per cycle that is flue gas DA. _CO2 = amount of air _CO2 captured per cycle FGCAPEX = pure carb run Flue gas operating costs in the form, i.e., if a mixture of ambient air and flue gas is supplied to each capture structure, M* = total natural gas burned in MMBTu M = available heat and Electricity generated COGENE = combined heat and power efficiency = M/M*
_FGCCO2 = flue gas _CO2 captured per year
DACCO2 = air _CO2 captured per _year
FTCO ₂ == total flue gas CO ₂ produced with J\11* natural gas burned
MTCO2 = total _CO2 captured per year = total _CO2 from flue gas and air captured per _year
ECF = efficiency of flue gas capture MDAC = energy per metric ton of trapped air _CO2 MFG = energy per metric ton of trapped flue gas _CO2 SHA = sensible heat of monolith array delta HR = Difference in heat of reaction between DAC CO ₂ site and flue gas CO ₂ site THF = total heat source in flue gas steam - sensible heat + CO ₂ reaction heat + water condensation heat - (Natural gas heat value is not constant please note)

These and other features of the present invention are set forth in, or are apparent from, the following detailed description and accompanying drawings.

FIG. 2 is a schematic top view of a pair of rotating multi-capture structure systems interacting to remove carbon dioxide from the atmosphere, for each loop and each group of capture structures, according to an exemplary embodiment of the present invention; Gradient level regeneration chambers are shown with two capture structures immediately upstream of each of the regeneration chambers shown within sealed housings that supply cleaned flue gas to the capture structures. It has a sealed conduit for

FIG. 2 is a schematic illustration of a pair of regeneration chambers for removing carbon dioxide from the capture structure of FIG. 1, including several inlet and outlet conduits connected to one of the chambers and a sealing conduit connecting the two A connecting conduit is shown.

FIG. 4 is a schematic of the regeneration chamber and flue gas trapping structure on each of the adjacent loops showing each chamber and the piping system configuration between the chambers.

Figures 13A-13C are schematic elevational views respectively showing the fans relatively stationary and rotating with each capture structure;

5 is a schematic side view of the dual induction shaft fan and plenum design of FIG. 4; FIG.

1 is a schematic elevational view of one of the interacting pairs of a rotating multi-capture structure system with a track-level regeneration chamber for removing carbon dioxide from the atmosphere and a flue gas stream for _CO2 capture; FIG. Figure 2 shows two capture structure housings just before processing.

1 is a schematic diagram showing the general operation of this system between the final adsorption stage and the _CO2 desorption regeneration step, showing a system in which all of the adsorption stages treat ambient air; FIG.

1 is a conceptual diagram showing the general operation between the final adsorption flue gas stage and the _CO2 desorption regeneration step of one of the inventively preferred embodiments of the system, which in this embodiment is referred to as "desorption The last adsorption stage immediately upstream of the unit, e.g. the 9th stage, receives flue gas pure or mixed with ambient air, the next preceding stage, e.g. exhaust, a mixture of that exhaust and ambient air, or ambient air only, depending on the composition of the ninth stage exhaust.

FIG. 2 is a conceptual diagram showing the general operation between the final adsorption mixed air flue gas stage and the _CO2 desorption and regeneration step of another preferred embodiment of the present invention of the system, in this embodiment: A final adsorption stage, for example the ninth stage, immediately upstream of the "desorption unit" receives flue gas mixed with ambient air.

within the desorption unit or out of the flue gas adsorption unit housing as each of the housings is at a graded level and each capture structure moves along the track and each capture structure enters each housing. FIG. 11 shows an example of a seal extending around all sides of each capture unit in one; FIG.

More Detailed Description of the Present Embodiment of the Invention A simplified depiction of the design of a system that performs these operations described above is shown in FIGS. 1-6. A detailed description of the maneuvers and ancillary equipment required are described below and are similar to those shown in common U.S. Pat. Nos. 10,413,866 and 10,512,880. .

In this embodiment, there are ten "capture structures". The capture structures are preferably, but not exclusively, placed in a decagonal configuration and placed on substantially circular or arcuate tracks. There are two substantially circular (or oval)/decagonal assemblies associated with each processing unit and they interact as shown. In this preferred embodiment, air is forced through the capture structure by an induced draft fan located inside the capture structure. At one location, the capture structures are located adjacent to a single sealed chamber box into which each capture structure is inserted as it moves along the track for processing. In a closed regeneration chamber box they are heated to a temperature of 130°C or less, more preferably 120°C or less, optimally 100°C or less, preferably with treated hot steam to release the _CO2 from the adsorbent. Regenerate the adsorbent. Alternatively, the regeneration chamber can be above or below the gradient. In this embodiment, the _CO2 adsorption time by the capture structure is preferably ten times longer than the adsorbent regeneration time.

While it is preferred to use a porous monolithic substrate in the capture structure, it is possible to use porous particles, i.e. a stationary bed of particulate material, supported within a frame on the capture structure. Please understand. In either case, the porous substrate preferably supports an amine sorbent for _CO2 when the particle capture structure has the same pore volume as the monolithic capture structure for supporting the sorbent.

The schematic diagram illustrates the basic operating concept of the system according to the invention. There are ten "capturing structures" 21,22 each mounted in a decagonal assembly configuration and movably supported on circular tracks 31,33. There are two circular/decagonal assemblies, A and B, associated with each processing unit, which interact. Air or flue gas is passed through each of the capture structures 21, 22 by induced draft fans 23, 26 located radially inward of each of the decagon assemblies and out of the system from the inner perimeter of each capture structure. Inducing a flow of exhaust gas in the away direction. At one position along the tracks 31,33 the capture structures 21,22 are adjacent to the closed recycle boxes 25,27 and the capture structures 21,22 make one revolution about the track. After it is completed, it is inserted into it for playback processing.

Thus, as shown in Figures 1 and 2, the first capture structure 21 is rotated to a position within the regeneration box 25 for processing. It is for the regeneration box 25 on the gradient. When the capture structures are in position within the play box 25, movement along the track is stopped for all of the capture structures. Alternatively, continue by increasing the track diameter and trapping structure and by having a suitable sealing system on the regeneration box and optional flue gas adsorption housing (121, 221, 122, 222). movement becomes possible. When the capture structures 21, 22 are regenerated and all of the capture structures are displaced, the regenerated capture structures are displaced from the regeneration boxes 25, 27 as shown in FIG. After the structures 21, 22 have treated the flue gas, they can be moved. This process is repeated substantially continuously. In the preferred embodiment shown in the drawings, one or more of the capture structures on each track move from the flue gas adsorption housing (121, 221, 122, 222). The timing preferably coincides with the timing of flue gas desorption. Alternatively, movement of the capture structure may be stopped each time the capture structure enters the regeneration box and one or more flue gas adsorption housings (121, 221, 122, 222). Transfer is then resumed when desorption and flue gas adsorption are complete.

However, as explained above, the present process invention is a low temperature (preferably ambient to 100° C.), semi-continuous process with unidirectional mass transport during each phase of the process. In a further novel aspect of this process, the reaction that captures _CO2 from the gas mixture takes place on a renewable material (in one preferred embodiment on aminopolymers) and the renewable material, e.g. It preferably occurs impregnated within the base material.

In preferred embodiments, the sorbent-bearing capture structures comprise a monolithic substrate that is in turn supported by a framework to form each capture structure.

Although the two decagon ring assemblies are interoperable, the capture structures for each decagon ring are moved in and out of their desorption/regeneration boxes at slightly different times, as described below. This makes it possible, for example, to pass heat between the boxes 25 and 27 to preheat the other box, for example the regeneration box 27, when the regeneration in the box 25 is completed. This saves heat at the start of regeneration and reduces the cost of cooling the capture structure after regeneration.

Three locations are available for the regeneration boxes 25, 27: above or below the rotating capture structure, or at a slope level, which does not allow continuous movement. See U.S. Pat. Nos. 10,413,866 and 10,512,880.

Regeneration Chamber 3 27 is mounted on the gradient of the rotating capture structure assembly. The box is similarly installed on a slope with adequate accessibility for maintenance and process piping. Suitable mutual sealing surfaces are placed on the box and on each capture structure such that when the capture structure is moved into position within the box, the movement is upward into the regeneration box on the rise. Or, whether downward into the regeneration box below grade, or straight into the regeneration box on grade, box 327 is sealed. The same is true for embodiments in which the flue gas adsorption housing (121, 221, 122, 222) can be on-grade or below or above the slope. There is also an optional closed chamber for the immediately preceding position along the track to feed flue gas or partially cleaned flue gas into the capture structure.

In all cases, the ancillary equipment (pumps, control systems, etc.) is preferably installed on the slope inside or outside the circumference of the track supporting the rotating capture structure assembly 39 .

The regeneration box and housing may be installed at different levels in particular situations without departing from the concept or scope of the present invention.

An alternative design within the scope of the present invention provides a system in which a pair of regeneration boxes, chambers 25, can move along a track. This is optimal if the track design allows for reciprocating motion by the capture structure along a straight track so that the play boxes 25 are not widely separated. Compared to existing disclosed devices in the prior art, this is as follows.
Minimize structural steel.
Locate all major equipment at grade level, except for the regeneration box, which serves only as a containment vessel.
Ensure that if the box is at a different level than the track, it does not interfere with the air flow to the capture structure.
Rotate all of the capture structures to prevent movement of the larger multi-unit system moving them into the regeneration box.
It allows the two regeneration boxes to be adjacent with a minimal gap to allow for the desired heat exchange for increased efficiency.

Mechanical actions with the necessary machinery and power include:
Rotating the two sets of capture structure assemblies about substantially circular tracks on the support structure and precisely positioning the components to positions where the capture structures are stopped, the capture structures are placed in the regeneration box and Securely and freely moves in and out of any flue gas adsorption housing.
The capture structure or substrate alone is removed, the capture structure is inserted into the regeneration box, the capture structure is removed from the regeneration box, and the capture structure is reinserted in its position on the track assembly. All of these movements occur vertically or alternatively as part of a horizontal rotational movement on the track. The capture structure and regeneration box are designed such that for vertically movable capture structures there is a substantially airtight seal between the top or bottom of each of the capture structures and the support structure of the box. be done. Seals can be on the sides as well as on the top and bottom for slopes of such regeneration boxes or flue gas adsorption housings. Alternatively, there may be a sealed door that closes when the capture structure moves into the regeneration box or flue gas adsorption housing. Examples of several conceptual designs of such seals are shown in the previously issued US Eisenberger patent and FIG. 10 of this application.

In all cases of one preferred embodiment, referring to FIGS. 1-9, the capture structure 21-1 (Ring A) is rotated into position and then regenerated or detached for processing, box 25. is moved to The pressure in the desorption box 25 (which houses the capture structure 21-1, ring A) is reduced to below 0.2 bar, for example using a vacuum pump 230. Box 25 is heated with steam at atmospheric pressure via line 235 . CO ₂ is produced from capture structure 21-1 and removed via outlet line 237 from box 25 for CO ₂ and condensate separated on condenser 240 (FIG. 3 ). Capture structure 22-1 (Ring B) is then placed in Box 27 (Ring B) while Box 25 is being processed, as described above (FIG. 3 ). The steam supply to box 25 is stopped and the _CO2 and condensate outlet lines are isolated. Boxes 25 and 27 are connected by opening valve 126 in connecting line 125 (FIG. 3 ).

The pressure within box 27 is reduced using vacuum pump 330 associated with box 27 . This reduces the system pressure in both boxes and draws the residual vapor and inert elements in box 25 through box 27 and then to the vacuum pump. This cools the box 25 (and therefore the trapping structure 21-1, ring A) to a lower temperature (i.e., the saturation temperature at the partial pressure of the vapor in the box) such that the trapping structure 21-1 Reduces the potential for oxygen deactivation of the adsorbent when placed back into the air stream. This process also preheats box 27 (and therefore capture structure 22-1, ring B) from ambient temperature to saturation temperature at the partial pressure of the vapor in box 25. FIG. Thus, energy is recovered and the amount of atmospheric pressure steam required to heat the second box 27 (capture structure 22-1 ring B) is reduced (FIG. 3 ). As the vacuum pump 330 reduces the pressure in boxes 25 and 27, the temperature of the first box 25 drops (from approximately 100°C to some intermediate temperature) and the temperature of the second box 27 drops (from the ambient temperature to the same intermediate temperature). CO ₂ and inert gases are removed from the system by vacuum pump 330 .

A valve between the first box 25 and the second box 27 is closed to isolate the boxes from each other. The capture structure 21-1 ring A is cooled to a temperature below that at which oxygen deactivation of the adsorbent is a concern when the capture structure is placed back into the air stream. Since the second box 27 and the capture structure 22-1, ring B are preheated, the amount of steam required to heat the box and capture structure is reduced . Capture structure 21-1 ring A is then moved into the capture structure assembly. The ring A capture structure assembly is rotated by one capture structure, then capture structure 21-2 ring A is inserted into box 25 ready for preheating. Box 27 is heated with atmospheric steam to recover the stripped _CO2 .

When the second box 27 (which houses the capture structure 22-1 ring B) is fully regenerated, the steam supply to box B is isolated and the _CO2 and condensate lines are connected using valves 241, 242. separated by The valve 126 between the first box 25 and the second box 27 is opened and the pressure in boxes 25,27 is reduced using the vacuum pump 230 system for box 25. The temperature of the second box 27 (and hence the trapping structure 22-1, ring B) is reduced (see 5 above). The temperature of the first box 25 (which houses the capture structure 21-2, ring A) is increased (see 5 above) (FIG. 5G). A vacuum pump 230 reduces the pressure in boxes 25,27. The temperature in box 25 drops (from approximately 100°C to some intermediate temperature). The temperature in box 27 rises (from ambient to the same intermediate temperature). CO ₂ and inert gases are removed from the system by vacuum pump 230 . The capture structure 22-1, ring B, is moved back into the ring assembly and the assembly rotates one bed. Capture structure 22 - 2 , ring B, is then inserted into box 27 . Box 25 (containing capture structure 21-2 ring A) is heated with atmospheric steam to release CO ₂ and regenerate the adsorbent (FIG. 5H). Preheating of box 27 then takes place as described above. This process is repeated for every bed as the decagon rotates many times.

When dealing with the preferred embodiment shown in Figure 8, in which both rings comprise a pair of flue gas adsorption housings just before entering the regeneration box, a supply of pretreated flue gas is preferably provided. For example, the ninth adsorption stage immediately prior to the regeneration box contains pretreated flue gas, or a mixture of pretreated flue gas and ambient air, typically having about 10-15% CO ₂ . either supplied. The exhaust from that stage can contain, for example, 2-8% CO ₂ . Preferably, when the upper range of _CO2 is vented, most preferably the exhaust gas is further adsorbed through the housing of the immediately preceding desorption stage to reduce the exhaust gas to a suitable level for venting to the atmosphere.

Preferred Design Parameters The current preferred basic principles for system design are as follows.
Weight of each captured structure to move:
1,500-10,000lbs. (including support structure)
Approximate bed size: Width: 5-6 meters Height: 9-10 meters Depth: 0.15-1 meter

It should be noted that the size of the capture structures may be adjusted depending on the specific conditions and desired or achievable processing parameters at each pair of geographic locations in the system.

For a system with 10 capture structures in each decagonal ring, the preferred outer system size of circular/decagonal structures is about 15-17 meters, preferably about 16.5 meters. The capture structure support structures may be driven individually along the track by, for example, electric motors and drive wheels. Alternatively, the support structure may be fixed to a single large motor that is used to drive specific locations along the track and all structures around the track and closed loop. In either case, the play box is placed in one location and all of the structures can stop their movement when one of the support structures is placed to be moved into the play box. . The economics of a single drive motor or engine, or multiple drive motors or engines, depends on many factors such as location and whether the drive is accomplished by an electric motor or by several fuel-driven engines. Dependent. The nature of the drive unit per se is not a primary feature of the invention and many are well known to those skilled in the art. Examples of suitable engines include, for example, internal or external combustion or gas pressure driven engines, process steam engines, or hydraulic or pneumatic engines operating using the Stirling engine cycle.

If the regeneration box is installed above track level, the top is approximately 20 meters above track level. If the regeneration box is installed below the slope of the track, the top of the box is just below the slope of the track. The box on the gradient is placed at a minimum height above the top of the trapping structure in order to completely contain the trapping structure within the box during regeneration.

If the regeneration box is not on an incline, the lift system for moving the capture structure into and out of the regeneration box should move in and out of the box for a period of time in the range of 30 seconds to 120 seconds, preferably 30 seconds to 45 seconds. should be able to achieve a move to Shorter periods allow greater flexibility in processing parameters. It is recognized that moving large capture structures has certain inherent mechanical limitations. One advantage of having the play box on a gradient is that no vertical movement is required. The capture structure simply rotates and seals into the box as part of the rotational motion, thus avoiding the vertical movement, lost time, and additional capital cost of the elevator. In either case, the two edges of the capture structure are solid and form a seal with the edge of the regeneration box.

U.S. Patent Application No. 13/098,370 (now U.S. Patent Application No. 8,500,855) U.S. Patent Application No. 9,925,488

Claims (20)

A system for removing carbon dioxide from a carbon dioxide-containing gas mixture comprising: a group of carbon dioxide removal structures, each removal structure within each group being supported on said structure; each porous substrate having an adsorbent supported within its pores, the adsorbent adsorbing or binding carbon dioxide to remove the carbon dioxide from the gas mixture. a group of carbon dioxide removal structures and an infinite loop support for said group of carbon dioxide removal structures, said infinite loop support following a closed curve while being exposed to a flow of a carbon dioxide-containing gas mixture. an infinite loop support arranged to allow movement of each group of said removal structures, and a position along said infinite loop support at which one removal structure may be sealingly mounted. wherein carbon dioxide adsorbed by said sorbent is stripped and captured from said sorbent when the removal structure is sealed in place therein and said sorbent is regenerated. and a sealed regeneration box, wherein said removal structure is positioned such that said adsorbent is exposed to a flow of a carbon dioxide-containing gas mixture to enable removal of _CO2 from said gas mixture. Each of the bodies supports the porous substrate, and the number of removal structures relative to the number of regeneration boxes determines the adsorption time (to remove _CO2 from the gas mixture) and the adsorption time (on the porous substrate). (to strip _CO2 from the adsorbent) and the regeneration time, the adsorption time is determined directly by the ratio of _CO2 from the gas mixture onto the adsorbent from the base level of the adsorbent to the desired is the time to adsorb to a level, the regeneration time is the time to strip the _CO2 until the desired level on the adsorbent returns to the base level, and the system is positioned one position along the track. further comprising a first chamber in, said first chamber designed to sealingly house each capture structure moving along said track;
an inlet designed for said first chamber to be connected to a source of CO2 _- containing flue gas, and a _CO2 purification flue after at least a portion of said _CO2 has been adsorbed by said adsorbent. and an outlet for gas. 2. The system of claim 1, wherein the first chamber is installed immediately adjacent to the regeneration box. 2. The method of claim 1, wherein the first chamber is designed to seal the capture structure within the first chamber when the flue gas is flowed into the first chamber. system. further comprising a combination of a seal located inside said first chamber and a seal located outside each of said capture structures, said combination of seals allowing flue gas to escape from within said first chamber; 2. The system of claim 1, wherein the system is designed to seal the capture structure within the first chamber to prevent leakage of . further comprising a second chamber at a position along the track upstream of the first chamber;
2. The system of claim 1, wherein the second chamber is designed to sealingly contain each capture structure traveling along the track before entering the first chamber. further comprising a valved conduit designed to connect said outlet from said first chamber to said inlet to said second chamber; 6. The system of claim 5, designed to be exposed to any CO2 _- purified flue gas exiting the chamber. each carbon dioxide removal structure in a second group, each respective removal structure in each group comprising a porous solid substrate supported on said removal structure, each porous substrate has an adsorbent supported within its pores, said adsorbent is capable of adsorbing or binding carbon dioxide to remove it from a gas mixture a removal structure;
a second infinite loop support for the second group of removal structures, the second infinite loop support aligning the respective removal structures of the second group along a closed curve A second infinite loop support, arranged to allow movement of a second infinite loop support, and a first removal structure at a position along each of said infinite loop supports, wherein one removal structure may be sealingly arranged. 2 sealed regeneration boxes wherein carbon dioxide adsorbed on said adsorbent is stripped and captured from said adsorbent when one removal structure is sealed in place therein; a second sealed regeneration box in which is regenerated, said sealed regeneration box further comprising a sealed conduit connecting said regeneration box to a source of process vapor, said conduit connecting said regeneration connected to an exhaust pump for removing gas from the box, each of said second group of removal structures exposing at least one major surface of said substrate to a flow of a carbon dioxide-containing gas mixture; outside the regeneration box, wherein the opposite major surface of the material is directly exposed to the atmosphere and the sorbent is capable of removing _CO2 from the gas mixture when exposed to a flow of a carbon dioxide-containing gas mixture. Supporting porous substrates at positions along a closed-loop support, the number of removal structures relative to the number of regeneration boxes is the adsorption time (to remove _CO2 from the gas mixture) and the porous The adsorption time is determined directly by the ratio of the regeneration time (to strip _CO2 from the adsorbent on the substrate) to the _CO2 from the gas mixture onto the adsorbent and the base level of the adsorbent. 2. The system of claim 1, wherein the regeneration time is the time to strip the _CO2 until the desired level on the adsorbent returns to the base level. 8. The system of claim 7, wherein the two groups of carbon dioxide removal structures are substantially identical to each other. a sealed fluid connection between each regeneration box and an exhaust pump for reducing the atmospheric pressure within the sealed regeneration box after the removal structure is sealed within the regeneration box; and the regeneration box. and a source of process heat steam for each regeneration box; and a sealed fluid connection between each regeneration box and the _CO2 recovery chamber. ,
The rotational motion of each of the two groups of carbon dioxide removal structures is entered by the other carbon dioxide removal structure of the regeneration box after regeneration of one of the carbon dioxide removal structures of the regeneration box is initiated. 9. The system of claim 8, wherein the offset is such that 10. The system of claim 9, wherein said adsorbent is a polymeric amine. A method of removing carbon dioxide from a carbon dioxide containing gas mixture comprising moving a group of respective carbon dioxide removal structures around a closed infinite loop while being exposed to a flow of said carbon dioxide containing gas mixture. wherein each removal structure in said group comprises a porous solid substrate supported on said structure, each porous substrate having an adsorbent supported within its pores; The adsorbent is capable of adsorbing or binding carbon dioxide and removing carbon dioxide from the gas mixture during the adsorption time, moving and a removal structure in place therein. along the endless loop support such that, when sealed, carbon dioxide adsorbed on the adsorbent is removed from the adsorbent and captured, and the adsorbent is regenerated during a regeneration time. sealingly disposing a carbon dioxide removal structure within a regeneration box at one location, each of said removal structures supporting said porous substrate on said closed infinite loop; except when the body is placed in the regeneration box, such that the adsorbent is continuously exposed to a flow of a carbon dioxide-containing gas mixture so as to allow removal of _CO2 from the gas mixture. In an internal position, when the removal structure is positioned within the regeneration box, the adsorbent is exposed to process heat at a temperature below 130° C. to strip the _CO2 from the adsorbent, and The number of removal structures relative to the number of regeneration boxes is directly determined by the ratio of the adsorption time to the regeneration time, the adsorption time being the length of time each structure is exposed to the flow of the carbon dioxide-containing gas mixture. is the time to adsorb _CO2 from the gas mixture on the sorbent from a base level on the sorbent to the desired level during which the regeneration time is the time the structures are in the regeneration box. is a time to adsorb _CO2 on the adsorbent until the desired level on the adsorbent returns to the base level;
The method comprises flowing CO2 _- containing flue gas into a first chamber positioned along the track, the first chamber passing through each capture structure moving along the track. the adsorbent hermetically containing and within the porous substrate on the capture structure adsorbs and removes carbon dioxide from the flue gas during an adsorption time; and passing said CO2 _- purified flue gas from said first chamber prior to moving said capture structure from said first chamber along. 12. The method of claim 11, wherein the first chamber is positioned immediately adjacent to the regeneration box. further providing a second chamber located along the track upstream of the first chamber;
13. The method of claim 12, wherein said second chamber sealingly houses each capture structure that moves along said track before entering said first chamber. A conduit designed to connect the outlet from the first chamber and the inlet to the second chamber is provided to move the capture structure in the second chamber to the first chamber. 14. The method of claim 13, further comprising exposing to any CO2 _- purified flue gas discharged from the chamber of. providing a second group of removal structures and a second moving infinite loop for supporting said second group, each of which moves around said second closed infinite loop; Each removal structure in the group comprises a porous solid substrate supported by each of said removal structures, each porous substrate having an adsorbent supported within its pores, said adsorbent comprising providing, capable of adsorbing or binding carbon dioxide;
exposing each respective carbon dioxide removal structure to a flow of said carbon dioxide _- containing gas mixture during an adsorption time to remove carbon dioxide from said gas mixture; each of said removal structures supporting said porous substrate on each of its closed infinite loops in a position such that said adsorbent is exposed to the flow of a carbon dioxide-containing gas mixture so as to enable There is removing and
providing a play box adjacent to each loop in one location;
sealingly placing one of said carbon dioxide removal structures sequentially in a regeneration box at one location along each of said infinite loop supports;
so that when one removal structure is sealed in place therein, the carbon dioxide adsorbed on the sorbent is stripped and captured from the sorbent, and the sorbent is regenerated; exposing the adsorbent to treatment heat at a temperature below 130° C. to strip _CO2 from the adsorbent on each removal structure hermetically disposed within each regeneration box during a regeneration period. ,
The number of removal structures provided in each loop is directly proportional to and determined by the ratio of the adsorption time to the regeneration time relative to the number of regeneration boxes provided adjacent each loop. , the adsorption time is the time to adsorb _CO2 from the gas mixture on the adsorbent from a base level on the adsorbent to a desired level, and the regeneration time is the time to adsorb the desired level on the adsorbent. 13. The method of claim 12, wherein the time to strip the _CO2 on the adsorbent until the <RTIgt; 16. The method of claim 15, further comprising reducing atmospheric pressure within each sealed regeneration box after removal structures are sealed within the regeneration box. passing the treated hot steam through the regeneration box to strip the _CO2 after the atmospheric pressure in the regeneration box is reduced; and stripping the stripped _CO2 from the regeneration box into a _CO2 recovery chamber. 17. The method of claim 16, further comprising: passing. one of the two groups of carbon dioxide removal structure groups has an adjacent first regeneration box, and the other of the two groups of carbon dioxide removal structure groups has an adjacent second regeneration box; The method comprises: after regeneration of the carbon dioxide removal structures in the first regeneration box has begun, the two groups of carbon dioxide removal structures enter the second one of the regeneration boxes. offsetting the rotational movement of each of the carbon dioxide removal structures;
reducing the atmospheric pressure in the other regeneration box to a preset pressure; opening a sealed connection and withdrawing residual vapor in the first regeneration box to preheat the second regeneration box and cool the removal structure in the first regeneration box; returning the cooled removal structure from the first regeneration box onto the infinite loop; and moving the removal structure around the infinite loop and periodically re-entering the regeneration box. 20. The method of claim 19, further comprising continuing the cycle to . The process heat is added to the regeneration box in the form of process hot steam, and when regeneration is complete in each of the regeneration boxes, steam remains in that box to preset the atmospheric pressure in the other r-boxes. and after completing the designated regeneration of the removal structure in the first regeneration box, opening the sealed connection between the two regeneration boxes; withdrawing residual steam in the regeneration box to preheat the second regeneration box and cool the removal structure in the first regeneration box; and continuing this cycle as the removal structure moves around the infinite loop and cyclically re-enters the regeneration box; 18. The method of claim 17, comprising: The treated hot steam enters each regeneration box at a temperature of about 120° C. or less, the second regeneration box is preheated to a temperature of about 60° C. or less, and the first regeneration box is heated to a temperature of about 60° C. or less. 20. The method of claim 19, cooled to a temperature below the temperature at which it is activated.

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